Linear-regioselective hydromethoxycarbonylation of styrene using Ru-clusters/CeO2 catalyst

作     者：Jinghua An Yehong Wang Zhixin Zhang Jian Zhang Martin Gocyla Rafal EDunin-Borkowski Feng Wang 安静华;王业红;张志鑫;张健;Martin Gocyla;Rafal EDunin-Borkowski;王峰

作者机构：State Key Laboratory of CatalysisDalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of SciencesBeijing 100049China Ernst Ruska Centre for Microscopy and Spectroscopy with Electrons and Peter Grünberg InstituteForschungszentrum Juelich GmbHJuelich 52425Germany 

基　　金：中国科学院战略性先导科技专项(XDB17020300) 国家自然科学基金(21721004,21690084,21690080) 

出 版 物：《Chinese Journal of Catalysis》 (催化学报（英文）)

年 卷 期：2020年第41卷第6期

页      码：963-969页

摘      要：Hydroalkoxycarbonylation of olefins has been considered to be one of the most attractive methods to synthesize esters. Controlling the regioselectivities of linear esters(L) and branched esters(B) is a challenging project for researchers working in this reaction. Although most of the attention has been paid to control the regioselectivity through ligand design in homogeneous catalytic systems, study in the area is still limited. Herein, Ru-clusters/CeO2 is employed as a heterogeneous catalyst for the hydromethoxycarbonylation of styrene without any additives. After optimization of the reaction conditions, the conversion of styrene is > 99% with 83% and 12% regioselectivity of linear and branched ester, respectively. By using different supports(CeO2(nanoparticle), CeO2-rod, and CeO2-cube), three catalysts including Ru-clusters/CeO2, Ru/CeO2-rod, and Ru/CeO2-cube are prepared and applied in the reaction. Structural characterizations demonstrate that the L/B ratio is related to the Ru size of supported Ru catalysts. Further Raman characterization and NH3-TPD demonstrate that the metal-support interaction and the concentration of oxygen vacancy of the catalyst have a great influence on the Ru size. The mechanism and kinetic analysis for this reaction are also investigated in this work.

主 题 词：Regioselectivity Ru-clusters/CeO2 Ester Hydromethoxycarbonylation Olefins Heterogeneous catalysis 

学科分类：081704[081704] 07[理学] 08[工学] 0817[工学-轻工类] 070303[070303] 0703[理学-化学类] 

核心收录：

D　O　I：10.1016/S1872-2067(19)63527-8

馆 藏 号：203878714...